Recent experiments have revealed ultrastrong coupling between light and matter as a promising avenue for modifying material properties, such as electrical transport, chemical reaction rates, and even superconductivity. Here, we explore (ultra)strong coupling as a means for manipulating the optical response of metamaterials based on ensembles of constituent units individually in the ultrastrong-coupling regime. We develop a framework based on linear response for quantum electrodynamical systems to study how light-matter coupling affects the optical response. We begin by applying this framework to find the optical response of a two-level emitter coupled to a single cavity mode, which could be seen as a ``meta-atom'' of a metamaterial built from repeated units of this system. We find optical behavior ranging from that of a simple two-level system (Lorentz-oscillator) to effectively transparent, as the coupling goes from the weak to deep strong-coupling regimes. We explore a one-dimensional chain of these meta-atoms, demonstrating the tunability of its optical behavior. Our scheme may ultimately provide a framework for designing metamaterials with low-loss, highly confined modes, as well as tunable (single-photon) nonlinearities.
Recent experiments have revealed ultrastrong coupling between light and matter as a promising avenue for modifying material properties, such as electrical transport, chemical reaction rates, and even superconductivity. Here, we explore (ultra)strong coupling as a means for manipulating the optical response of metamaterials based on ensembles of constituent units individually in the ultrastrong-coupling regime. We develop a framework based on linear response for quantum electrodynamical systems to study how light-matter coupling affects the optical response. We begin by applying this framework to find the optical response of a two-level emitter coupled to a single cavity mode, which could be seen as a ``meta-atom'' of a metamaterial built from repeated units of this system. We find optical behavior ranging from that of a simple two-level system (Lorentz-oscillator) to effectively transparent, as the coupling goes from the weak to deep strong-coupling regimes. We explore a one-dimensional chain of these meta-atoms, demonstrating the tunability of its optical behavior. Our scheme may ultimately provide a framework for designing metamaterials with low-loss, highly confined modes, as well as tunable (single-photon) nonlinearities.
Harnessing the interaction between light and matter at the quantum level has been a central theme in atomic physics and quantum optics, with applications from quantum computation to quantum metrology. Combining complex interactions with photonic synthetic materials provides an opportunity to investigate novel quantum phases and phenomena, establishing interesting connections to condensed matter physics. Here we explore many-body phenomena with a single artificial atom coupled to the many discrete modes of a photonic crystal. This experiment reaches the ultrastrong light-matter coupling regime using the circuit quantum electrodynamics paradigm, by galvanically coupling a highly nonlinear fluxonium qubit to a tight-binding lattice of microwave resonators. In this regime, the transport of a single photon becomes a many-body problem, owing to the strong participation of multi-photon bound states arising from interactions that break particle number conservation. Exploiting the effective photon-photon interactions mediated by the qubit, the transport of multiple photons leads to complex multimode dynamics that can be employed for generating a continuous reservoir of strongly-correlated photons, an important resource for quantum networks. This work opens exciting prospects for exploring nonlinear quantum optics at the single-photon level and stabilizing entangled many-body phases of light.
When in a quantum optical system the coupling between matter and cavity mode becomes comparable to the bare excitation frequency, we enter a non-perturbative coupling regime, as perturbation theory fails describing the system’s dynamics. While recent advances in Cavity Quantum Electrodynamics allowed to achieve very high values of the coupling strength, thanks to the resonators properties optimization and the employment of solid-state devices, an ever growing interest has been shown about the possibility of significantly modify materials’ properties. It has been demonstrated that the chemical structure of molecules strongly coupled to a photon mode can be altered, which opens the possibility to manipulate and control chemical reactions. The aim of this thesis is to explore non-perturbative regimes on several quantum systems, and to investigate the effects of the coupling upon their properties, such as internal degrees of freedom or electronic states structure. I first developed a novel theory to determine the polariton spectrum of a dipolar ensamble in which a Ising-like dipole-dipole interaction in the 2 non-perturbative regime is considered. A further important focus is the investigation of the saturation effects due to the inclusion of the inter-dipole interaction, and the interplay between the latter and light-matter coupling strength. I also explored specifically the influence of the coupling on the rotational degrees of freedom of an ensemble of two-dimensional freely rotating dipoles, all coupled to a single cavity mode, finding that they are driven by the collective light-matter coupling to undergo a crossover between an isotropic and an aligned phase. I then investigated the case of cavity-embedded doped quantum wells, demonstrating that not only it is possible to couple a discrete cavity mode and bound-to-continuum transitions, but also that a novel bound exciton state appears, induced by the coupling strength. This results shows how light–matter coupling can be used to tune both optical and electronic properties of semiconductor heterostructures beyond those permitted by mere crystal properties. Finally, I explored the physics of an array of THz metamaterial resonators coupled to cyclotron resonances of a two-dimensional electron gas, developing a multiple-mode theory that takes in account the interaction between multiple photon modes mediated by the electrons. My results show that this cross-interaction, due to the strong two-dimensional geometry of the optically active medium, leads to the hybridization of different uncoupled photon modes, and manifests as a visible change of the distribution of the coupled electromagnetic field.
The idea of making photons effectively interact has attracted a lot of interest in recent years, for several reasons. Firstly, since photons do not naturally interact with each other, it is of fundamental physical interest to see what kind of medium can mediate interactions between these fundamental and non-interacting particles, and to what extent. Secondly, photonics is a major candidate for future quantum technology, due to the easy manipulation, readout, and transport of photons, which makes them ideal for quantum information processing. Finally, achieving strong and tunable interactions among photons would open up an avenue for exploring the many-body physics of a fluid of light. In this thesis, we will see how a cavity formed of subwavelength lattices of two-level atoms can confine photons to a nonlinear environment for a long time, such that emitted photons have accumulated strong correlations both among their momenta and in their temporal statistics. This speaks of a strong photon-photon interaction within the cavity. The nonlinearity originates in the saturability of individual atoms, and the lattice structure results in a strong and low-loss collective interaction with light. While a single atomic lattice has a largely linear nature, as the effect of individual atoms washes out in the collective response, the confining geometry of the cavity means the photons are exposed to the underlying saturability of the atoms for such a long time that the nonlinearity is revived. We will analyse this system both using a standard input-output formalism, where the nonlinear physics of the system is handled numerically, and a powerful Green's function-based approach that allows for exact analytical results with no additional approximations. This analytical description has the potential to lead to an exact study of the many-body physics of interacting photons in a two-dimensional setting.
Dressing quantum states of matter with virtual photons can create exotic effects ranging from vacuum-field modified transport to polaritonic chemistry, and may drive strong squeezing or entanglement of light and matter modes. The established paradigm of cavity quantum electrodynamics focuses on resonant light-matter interaction to maximize the coupling strength ΩR/ωc, defined as the ratio of the vacuum Rabi frequency and the carrier frequency of light. Yet, the finite oscillator strength of a single electronic excitation sets a natural limit to ΩR/ωc. Here, we demonstrate a new regime of record-strong light-matter interaction which exploits the cooperative dipole moments of multiple, highly non-resonant magnetoplasmon modes specifically tailored by our metasurface. This multi-mode coupling creates an ultrabroadband spectrum of over 20 polaritons spanning 6 optical octaves, vacuum ground state populations exceeding 1 virtual excitation quantum for electronic and optical modes, and record coupling strengths equivalent to ΩR/ωc=3.19. The extreme interaction drives strongly subcycle exchange of vacuum energy between multiple bosonic modes akin to high-order nonlinearities otherwise reserved to strong-field physics, and entangles previously orthogonal electronic excitations solely via vacuum fluctuations of the common cavity mode. This offers avenues towards tailoring phase transitions by coupling otherwise non-interacting modes, merely by shaping the dielectric environment.
Ultrastrong coupling between light and matter has, in the past decade, transitioned from a theoretical idea to an experimental reality. It is a new regime of quantum light–matter interaction, which goes beyond weak and strong coupling to make the coupling strength comparable to the transition frequencies in the system. The achievement of weak and strong coupling has led to increased control of quantum systems and to applications such as lasers, quantum sensing, and quantum information processing. Here we review the theory of quantum systems with ultrastrong coupling, discussing entangled ground states with virtual excitations, new avenues for nonlinear optics, and connections to several important physical models. We also overview the multitude of experimental setups, including superconducting circuits, organic molecules, semiconductor polaritons, and optomechanical systems, that have now achieved ultrastrong coupling. We conclude by discussing the many potential applications that these achievements enable in physics and chemistry.